Transient dielectric function of gallium undergoing order-disorder phase transition induced by femtosecond laser pulses

The reflectivity of Gallium films excited by femtosecond laser can be raised from ~55% to up to ~85% on a picosecond time-scale. Temporal behavior of the reflectivity exhibits three clearly distinguished stages: an initial 2 - 4 ps sharp rise, a relatively slow increase to a maximum value in a few 100 ps, and afterwards a long slope in ~ (0.1 - 1) μs to the original value. In this paper we present reflectivity measurements in a pump-probe scheme with one pump and two identical simultaneous femtosecond probes set at two different angles, which completely determines the real and imaginary parts of the dielectric function with time resolution ~ 200 fs. The analysis of the experimental data uncovered a number of new phenomena: (1) the energy density threshold to initiate phase transition is several times lower than the equilibrium enthalpy of melting; (2) the initial 2 - 4 ps rise of reflectivity relates to the transformation to a new phase in the absence of energy loss due to cooling. The second, slower stage (~100 ps) relates to a heat conduction dominated process; (3) the rate of the reflectivity change strongly increases with the increase of the pump laser intensity; (4) the volume fraction of the new phase reaches only 60% even with the deposited energy exceeds more than two times the equilibrium enthalpy of melting; (5) the electron-to-lattice coupling rate is a transient non-linear function of temperature that is drastically different from the equilibrium conditions. The results suggest a mechanism to control of the reflectivity switching, and thus the duty cycle of the reversible phase transition (crystal-metal-crystal), through an optimal combination of the laser parameters, target and substrate material. As a result, new all-optical switching devices with ps-range switching time could be designed utilizing the nonlinear dielectric properties of the non-equilibrium solid-state plasma.